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Title: Structure-property relationship of metal-organic frameworks (MOFs) and physisorbed off-gas radionuclides.

Abstract

We report on the host-guest interactions between metal-organic frameworks (MOFs) with various profiles and highly polarizable molecules (iodine), with emphasis on identifying preferential sorption sites in these systems. Radioactive iodine 129I, along with other volatile radionuclides (3H, 14C, Xe and Kr), represents a relevant component in the off-gas resulted during nuclear fuel reprocessing. Due to its very long half-life, 15.7 x 106 years, and potential health risks in humans, its efficient capture and long-term storage is of great importance. The leading iodine capture technology to date is based on trapping iodine in silver-exchanged mordenite. Our interests are directed towards improving existent capturing technologies, along with developing novel materials and alternative waste forms. Herein we report the first study that systematically monitors iodine loading onto MOFs, an emerging new class of porous solid-state materials. In this context, MOFs are of particular interest as: (i) they serve as ideal high capacity storage media, (ii) they hold potential for the selective adsorption from complex streams, due to their high versatility and tunability. This work highlights studies on both newly developed in our lab, and known highly porous MOFs that all possess distinct characteristics (specific surface area, pore volume, pore size, and dimension ofmore » the window access to the pore). The materials were loaded to saturation, where elemental iodine was introduced from solution, as well as from vapor phase. Uptakes in the range of {approx}125-150 wt% I2 sorbed were achieved, indicating that these materials outperform all other solid adsorbents to date in terms of overall capacity. Additionally, the loaded materials can be efficiently encapsulated in stable waste forms, including as low temperature sintering glasses. Ongoing studies are focused on gathering qualitative information with respect to localizing the physisorbed iodine molecules within the frameworks: X-ray single-crystal analyses, in conjunction with high pressure differential pair distribution function (d-PDF) studies aimed to identify preferential sites in the pores, and improve MOFs robustness. Furthermore, durability studies on the iodine loaded MOFs and subsequent waste forms include thermal analyses, SEM/EDS elemental mapping, and leach-durability testing. We anticipate for this in-depth analysis to further aid the design of advanced materials, capable to address major hallmarks: safe capture, stability and durability over extended timeframes.« less

Authors:
;  [1]; ; ;  [1];
  1. Argonne National Laboratory
Publication Date:
Research Org.:
Sandia National Laboratories
Sponsoring Org.:
USDOE
OSTI Identifier:
1032941
Report Number(s):
SAND2010-8253C
TRN: US1200256
DOE Contract Number:  
AC04-94AL85000
Resource Type:
Conference
Resource Relation:
Conference: Proposed for presentation at the Fourth International Conference on Integration of Renewable and Distributed Energy Resources held December 6, 2010 in Albuquerque, NM.
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; ADSORBENTS; ADSORPTION; CAPACITY; DIMENSIONS; DISTRIBUTION FUNCTIONS; IODINE; MONITORS; MORDENITE; NUCLEAR FUELS; RADIOISOTOPES; REPROCESSING; SATURATION; SINTERING; SORPTION; STABILITY; STORAGE; SURFACE AREA; WASTE FORMS

Citation Formats

Nenoff, Tina Maria, Chupas, Peter J, Garino, Terry J, Rodriguez, Mark Andrew, Chapman, Karena W, and Sava, Dorina Florentina. Structure-property relationship of metal-organic frameworks (MOFs) and physisorbed off-gas radionuclides.. United States: N. p., 2010. Web.
Nenoff, Tina Maria, Chupas, Peter J, Garino, Terry J, Rodriguez, Mark Andrew, Chapman, Karena W, & Sava, Dorina Florentina. Structure-property relationship of metal-organic frameworks (MOFs) and physisorbed off-gas radionuclides.. United States.
Nenoff, Tina Maria, Chupas, Peter J, Garino, Terry J, Rodriguez, Mark Andrew, Chapman, Karena W, and Sava, Dorina Florentina. Mon . "Structure-property relationship of metal-organic frameworks (MOFs) and physisorbed off-gas radionuclides.". United States.
@article{osti_1032941,
title = {Structure-property relationship of metal-organic frameworks (MOFs) and physisorbed off-gas radionuclides.},
author = {Nenoff, Tina Maria and Chupas, Peter J and Garino, Terry J and Rodriguez, Mark Andrew and Chapman, Karena W and Sava, Dorina Florentina},
abstractNote = {We report on the host-guest interactions between metal-organic frameworks (MOFs) with various profiles and highly polarizable molecules (iodine), with emphasis on identifying preferential sorption sites in these systems. Radioactive iodine 129I, along with other volatile radionuclides (3H, 14C, Xe and Kr), represents a relevant component in the off-gas resulted during nuclear fuel reprocessing. Due to its very long half-life, 15.7 x 106 years, and potential health risks in humans, its efficient capture and long-term storage is of great importance. The leading iodine capture technology to date is based on trapping iodine in silver-exchanged mordenite. Our interests are directed towards improving existent capturing technologies, along with developing novel materials and alternative waste forms. Herein we report the first study that systematically monitors iodine loading onto MOFs, an emerging new class of porous solid-state materials. In this context, MOFs are of particular interest as: (i) they serve as ideal high capacity storage media, (ii) they hold potential for the selective adsorption from complex streams, due to their high versatility and tunability. This work highlights studies on both newly developed in our lab, and known highly porous MOFs that all possess distinct characteristics (specific surface area, pore volume, pore size, and dimension of the window access to the pore). The materials were loaded to saturation, where elemental iodine was introduced from solution, as well as from vapor phase. Uptakes in the range of {approx}125-150 wt% I2 sorbed were achieved, indicating that these materials outperform all other solid adsorbents to date in terms of overall capacity. Additionally, the loaded materials can be efficiently encapsulated in stable waste forms, including as low temperature sintering glasses. Ongoing studies are focused on gathering qualitative information with respect to localizing the physisorbed iodine molecules within the frameworks: X-ray single-crystal analyses, in conjunction with high pressure differential pair distribution function (d-PDF) studies aimed to identify preferential sites in the pores, and improve MOFs robustness. Furthermore, durability studies on the iodine loaded MOFs and subsequent waste forms include thermal analyses, SEM/EDS elemental mapping, and leach-durability testing. We anticipate for this in-depth analysis to further aid the design of advanced materials, capable to address major hallmarks: safe capture, stability and durability over extended timeframes.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2010},
month = {11}
}

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